INTRODUCTION Effects of road traffic on the ambient concentrations

Transkrypt

Annals of Warsaw University of Life Sciences – SGGW
Land Reclamation No 45 (2), 2013: 243–253
(Ann. Warsaw Univ. of Life Sci. – SGGW, Land Reclam. 45 (2), 2013)
Effects of road traffic on the ambient concentrations of three PM
fractions and their main components in a large Upper Silesian city
WIOLETTA ROGULA-KOZŁOWSKA, PATRYCJA ROGULA-KUPIEC,
BARBARA MATHEWS, KRZYSZTOF KLEJNOWSKI
Institute of Environmental Engineering of the Polish Academy of Sciences
Abstract: Effects of road traffic on the ambient
concentrations of three PM fractions and their
main components in a large Upper Silesian city.
The study concerns the assessment of the traffic influence on the concentrations of three particulate matter (PM) fractions and their basic
components. The PM samples were collected simultaneously at two receptors in Katowice. The
measurement sites represented the so-called urban
background and traffic points. The contents of the
organic and elementary carbon as well as water-soluble ions were determined in the samples. It
has been observed that the traffic (car engines)
pollution emissions enrich the submicron and fine
PM particles with the elementary carbon at a typical urban background in southern Poland. On the
other hand, the influence of the re-suspension of
the road and soil dust, caused by traffic, on the
concentrations and chemical composition is observed for the coarse PM fraction.
Key words: PM1, PM1-2.5, PM2.5-10, elemental carbon, organic carbon, chemical composition, size
distribution, traffic site, urban background
INTRODUCTION
Road traffic has a significant influence
on the environment. It also influences
pollutant concentrations in the air (e.g.
Versulis 1994, Morawska et al. 1999).
Dusts emitted from streets, crossroads or
motorways are mainly made of particles
emitted from cars. They also contain settled dust re-emitted from road and kerb
surfaces due to the traffic. The car engine
emissions tend to decrease owing to the
legal restrictions and devices designed to
clean flue gases (diesel particulate filters,
DPFs). For example, the research conducted in the Caldecott Tunnel (USA)
showed that the coefficient values for
the emission of particles with diameters
of up to 2.5 μm (PM2.5) declined. The
study (Ban-Weiss et al. 2008) indicates
that the values changed from 0.11 ±0.01
(g of PM2.5 per kg of fuel) in 1997 to
0.07 ±0.02 in 2006 for gasoline engines.
For the diesel ones, the values dropped
from 2.7 ±0.3 (g of PM2.5 per kg of fuel)
in 1997 to 1.4 ±0.3 in 2006.
The most detailed information on the
characteristics of the dust emitted from
cars can be obtained from the research
conducted in road tunnels. Such measurements were performed by Pierson
and Brachaczek in the mountain tunnels in Allegheny and Tuscarora (USA)
between 1970 and 1979. The researchers applied a complex set of apparatus
and methodologies. Their investigations
helped to identify the dust. Its main
sources were exhaust pipes, tyre and
brake lining abrasion and the soil particle re-emission. Only 3.5% of the dust
had an unknown origin. Approximately
80% of the particulate matter (PM) mass
was constituted by carbon compounds,
244
W. Rogula-Kozłowska et al.
mainly from heavy diesels (10–15% of
the whole traffic); sulphates made up
5%; inorganic matter from fuel and oil
made up 10%; tyres and soil particles
constituted 1% and 10%, respectively.
The studies conducted in road tunnels by Weingartner et al. (1997) in
1993, Kirchstetter et al. (1999) in 1997,
Allen et al. (2001) in 1999 and Geller
et al. (2005) in 2004 demonstrated that
carbon (both elemental and organic) had
the biggest percentage in the researched
PM masses.
Recently, the research on the influence that the traffic emission exerts on
the atmospheric air quality has been focused on the search for and evaluation
of the PM concentrations and chemical
compositions. The examinations have
been carried out at tunnels, street canyons, and surroundings of busy roads but
also at sites that are not under the influence of traffic.
The studies show that traffic is an
important source of the PM2.5 fraction
(Väkevä et al. 1999, Zhu et al. 2002,
Slezakowa et al. 2007). At some places,
it also contributes to the emission of the
coarse fraction – PM2.5-10, particles with
diameters of 2.5–10 μm (Hueglin et al.
2005).
The investigation undertaken in Switzerland demonstrates that the PM10 (particles with diameters of up to 10 μm)
increase at kerbsites reached 64% when
compared with the urban background.
However, the increase in PM2.5 was only
23% (Hueglin et al. 2005). On the other
hand, some studies estimate that the traffic emission constitutes at least 50% of
the PM2.5 mass (Harrison et al. 2004).
Hueglin et al. (2005) conducted one
of the first complex studies in Europe
that concerned the changes in the chemical composition of the aerosol under the
traffic emission influence. They found
out that sulphate and nitrate percentages
in the yearly concentrations of PM2.5 and
PM10 were higher in the rural, suburban
and urban background areas than at the
sites under the traffic influence (Hueglin et al. 2005). At the sites where the
traffic influence was heavy, the organic
matter (OM) and elemental carbon (EC)
had the biggest percentages in the yearly
concentrations of PM2.5 and PM10. EC
constituted around 14–18% of the PM
mass concentrations. Its percentage was
5–10% at the sites that were not under
the traffic emission influence (Hueglin
et al. 2005).
The traffic emission influence on the
physicochemical structure of the aerosol was also observed in the Upper Silesian urban area (Rogula-Kozłowska
et al. 2008, 2011). It was discovered in
the close vicinity of roads and crossroads.
Nonetheless, the research conducted so
far has concentrated on short-term measurements of the PM2.5 or PM10 concentrations. It has also concerned analyses
of the element compositions, but mainly
in the surface layer of the collected PM
samples. It has been concluded that, contrary to other regions, the PM concentrations in the Upper Silesian urban area are
still formed by the municipal and industrial sources. The traffic emission is less
important.
The following study evaluates the
traffic influence on the concentrations
and chemical compositions of three PM
fractions collected at the same time, i.e.
PM1, PM1-2.5, PM2.5-10 (particle diameters of up to 1, 1–2.5 and 2.5–10 μm,
respectively). The presented paper is
Effects of road traffic on the ambient concentrations of three PM...
a part of the first complex evaluation
of the traffic influence on the physicochemical properties of PM, including the
submicron fraction (PM1), carried out in
Poland.
MATERIAL AND METHODS
The PM samples were collected at two
sampling points in Katowice. One of the
points was located in the area meeting the
requirements of the Directive 2008/50/
/EC for locations representing the so-called urban background. According to
the Directive, such a point must represent inhabitants’ exposition to the ambient concentration in the residential areas
of larger urban agglomerations, in which
the air quality is mainly influenced by the
municipal and industrial emissions. The
site chosen for the research was located
in the vicinity of a large residential area
in the Muchowiec district. It was marked
with the TM symbol. The other point, i.e.
the so-called traffic point (marked with
the A4 symbol) was located in the area
directly influenced by the traffic emission. It was placed at the A4 motorway
kerb, approximately 1.5 km south of the
city centre.
The samples were collected in the
spring-summer season (mid-March to
mid-June 2012). The winter season was
excluded from the investigation due
to the increased municipal emission
of the PM (particularly carbon compounds) that could conceal the traffic
emission influence (Rogula-Kozłowska
et al. 2008, 2013). Each measurement
lasted around 1 week. The longest one
took 173 h, while the shortest one lasted
142 h. Altogether, 9 measurements were
performed.
245
Two thirteen-stage low-pressure impactors (DLPI, Dekati Low Pressure
Impactor) were used for the sampling.
DLPIs are used to determine the mass
distribution of the collected material (PM
and/or its components; in this case – carbon and ions present in the PM samples)
in relation to the particle size, for the particle diameter range of 0.03–10 μm and
at the flow rate of 30 l/min (Klejnowski
et al. 2010).
The PM samples were collected on
special substrates (nylon membranes or
quartz filters). Their masses were determined through weighing the substrates
on the Rawag microbalance (1-μg resolution) before and after the exposition.
Before and after the exposition, the
filters were conditioned in a weighing
room (48 h, relative air humidity 45
±5%, air temperature 20 ±2°C). All the
operations related to the impactor preparation for the examinations, including
the filter mounting onto the impactor
stages, were carried out in the sterile air
stream inside a laminar flow cabinet. After sampling in the field, the filters with
the PM were transferred into sterile glass
Petrie dishes in the laminar flow cabinet.
Immediately after the filters with the PM
were weighed, they were put into a refrigerator. They were kept there until the
analysis took place.
At both sampling points, the samples
were collected alternately (every second measurement) onto the quartz filters
(Whatman, QMA, ø 2.5 mm, CAT No.
1851-025) or nylon membranes (Whatman, Nylon Membrane Filters 0.2 μm,
ø 25 mm, Cat No. 7402-002). The samples deposited on the quartz filters were
analysed for the organic carbon (OC)
and EC contents. The samples collected
246
on the nylon membranes were extracted
in water. The water extracts were used to
determine the concentrations of the main
ions (Cl–, NO3–, SO42–, Na+, NH4+, K+,
Ca2+, Mg2+). The analytical procedures
and apparatus applied to the chemical
analysis of the samples were discussed
in detail in the paper (Rogula-Kozłowska
and Klejnowski 2013).
RESULTS
The PM1, PM1-2.5 and PM2.5-10 concentration values were similar at the A4 and
TM sampling points (Fig. 1, Table 1).
The visible increase (approx. 25%) in the
concentration at the A4 point in relation
to the TM one was observed only for the
coarse PM fraction (PM2.5-10). For the
submicron PM (PM1), only the 3-percentage increase was observed at motorway,
20
1800
18
A4
A4
1600
TM
TM
-3
1400
14
stĊĪenie, ng m
stĊĪenie, µ g m
-3
16
12
10
8
6
1200
1000
800
600
4
400
2
200
0
PM1
OC
0
EC
Na+
NH4+
K+
Ca2+
Mg2+
Cl-
NO3-
SO42-
400
6
A4
350
TM
stĊĪenie, ng m-3
stĊĪenie, µ g m-3
5
4
3
2
A4
TM
Mg2+
Cl-
300
250
200
150
100
1
50
0
PM1-2,5
OC
0
EC
Na+
5
A4
Ca2+
NO3-
SO42-
A4
TM
TM
200
-3
4
3.5
stĊĪenie, ng m
-3
K+
250
4.5
stĊĪenie, µ g m
NH4+
3
2.5
2
1.5
1
150
100
50
0.5
0
PM2,5-10
OC
EC
0
Na+
NH4+
K+
Ca2+
Mg2+
Cl-
NO3-
SO42-
FIGURE 1. Concentrations of PM1, PM1-2.5, PM2.5-10 and OC/EC bound to these fractions (on the left)
and concentrations of water-soluble ions (on the right) bound to PM1, PM1-2.5, PM2.5-10 at the A4 and
TM sampling points in Katowice
247
TABLE 1. The ratio of the PM concentration and its main components in three PM fractions at the A4
and TM sampling points
Fraction
PM
OC
EC
Na+
NH4+
K+
Ca2+
Mg2+
Cl–
NO3–
SO42–
PM1
1.03
1.00
2.80
0.73
0.97
0.68
0.53
–
1.01
0.97
0.93
PM1-2.5
0.97
0.97
1.82
1.01
1.00
1.24
0.50
–
0.96
0.95
0.97
PM2.5-10
1.25
1.27
1.76
1.84
0.71
2.80
2.20
–
1.28
0.94
0.95
when compared to the average value observed in the urban background. Nevertheless, the PM1 concentrations at both
sampling points were high even though
the measurements were carried out in the
warm season, when the PM concentrations in Poland are generally lower than
in the cold season (because of emission
and metrological/bioclimatic conditions,
e.g. Pastuszka et al. 2003, Klejnowski
et al. 2007, 2010, Juda-Rezler et al. 2011,
Majewski et al. 2011, Zwoździak et al.
2012, Majewski and Ćwiek 2013, Rogula-Kozłowska and Klejnowski 2013).
The sum of the average PM1 and PM1-2.5
(fine dust) concentrations was close to
the average permissible yearly value for
PM2.5 (25 μg/m3).
As it has been shown in the Introduction, the dust in the engine flue gases
contains EC particles, PAHs from incomplete fuel combustion, compounds
formed from the re-synthesis of fuel residues, and substances used as additives
to fuels and oils. The traffic emission
influence at the motorway demonstrated
itself through the visibly higher (for the
A4 point) EC concentrations. They were
nearly three times higher at the A4 than
the TM point. The EC concentrations
were nearly twice as high for the PM1-2.5
and PM2.5-10 fractions at the A4 point
(Table 1).
Contrary to other European locations,
EC was not mainly concentrated in the
submicron and fine PM (Fig. 1); at both
points in Katowice (Rogula-Kozłowska
et al. 2013). It also concerned the location that was directly exposed to the traffic emission. It seems possible that the
significant contribution of the municipal
emission to the EC balance in Katowice was responsible for the fact that
coarse particles (PM2.5-10) were enriched
with EC. Low-performance, obsolete
coal furnaces are used by Upper Silesian inhabitants to cook and heat water
throughout the year. Consequently, they
make emitters of large soot agglomerates from incomplete combustion. The
unusual increase in the PM2.5-10-related
EC concentrations at the traffic point
(in comparison with the corresponding
concentrations at the urban background
point) may be related to the fact that old
cars with faulty DPFs move along the
roads. As a result, large particles (soot
agglomerates) can be emitted.
In areas where traffic influences the
concentrations of the PM and its components, the road proximity causes
a decrease in the OC/EC ratio when compared to the values observed at sites far
afield from the roads (Rogula-Kozłowska
et al. 2013). The high OC/EC concentration ratio for the submicron and fine PM
(Fig. 1) can indicate that the A4 motorway
traffic volume and the fine EC particle
emission related to it are not high enough
to change the ratio value as it happens at
248
other similar locations. In Upper Silesian
cities and towns, the lower OC/EC ratio
is observed during the heating season, irrespective of the sampling point location
(Rogula-Kozłowska et al. in press).
For the coarse fraction (PM2.5-10), the
OC concentration was higher by 27%
at the A4 point than at the TM one. It is
probably related to the adsorption of organic compounds on the coarse – either
mineral or soot – PM particles (Seinfeld
and Pandis 2006). The OC concentrations were similar for the remaining fractions at both points (Fig. 1, Table 1).
The so-called secondary atmospheric
aerosol (NH4+, NO3–, SO42–) forms because of the photochemical transformations of the particle gas precursors (Seinfeld and Pandis 2006). The concentrations
of its components were similar at both
points (A4 and TM). For the PM2.5-10
fraction, the equivalent ion balance (Table 2) shows that the secondary inorganic aerosol (SIA) probably contained only
ammonium sulphate ((NH4)2SO4) at both
sampling points. The SIA contained both
ammonium sulphate and ammonium nitrate (NH4NO3) in PM1 and PM1-2.5.
The conclusions are drawn on the basis of the commonly used but highly simplified balancing of PM-related cations
and anions. Some studies reveal that the
atmospheric aerosol can have acidic pH
(due to the sulphuric acid presence) even
if the ratio of NH4+/SO42– mass equivalent is higher than 2 or even (i.e. SO42–/
/NH4+ ≤ 0.5 (Pathak et al. 2009, Huang
et al. 2011).
Low values of the ratio of total cation equivalent to total anion equivalent
(Σcations/Σanions, Table 2) at both sampling
points follow the findings on the possibly acidic pH of the aerosol in Katowice.
Consequently, the (NH4)2SO4 concentrations estimated with simple stoichiometric computations can be slightly inflated as the computations assume that
sulphates should react completely with
ammonium ions at NH4+/SO42– ≥ 1.
Low values of the ratio of total cation equivalent to total anion equivalent
(Σcations/Σanions) at both sampling points
(much lower than 1 for PM2.5-10) do not
TABLE 2. Equivalent ion balance and probable composition of the SIA composition in PM1, PM1-2.5,
PM2.5-10 at the A4 and TM points
Specification
PM1-2.5
0.92
0.87
PM2.5-10
PM1
PM1-2.5
0.73
0.95
0.84
A4
Σcations/Σanions [neqm–3/neqm–3]
a
PM1
–3
–3
PM2.5-10
TM
0.55
NR [neqm /neqm ]
1.08
0.96
0.32
1.06
0.93
0.42
SO42–/NH4+ [neqm–3/neqm–3]
0.57
0.58
1.59
0.59
0.59
1.20
[(NH4)2SO4]b [μgm–3]
1.98
0.50
0.14
2.12
0.51
0.20
[ex-NH4+]c [μgm–3]
0.40
0.10
0.00
0.40
0.10
0.00
1.79
0.45
0.00
1.77
0.43
0.00
[NH4NO3]d [μgm–3]
+
2–
–
a – NR = NH4 /(SO4 + NO3 ).
b – [(NH4)2SO4] = 1.38[SO42–] if SO42–/NH4+ < 1 and [(NH4)2SO4] = 3.67 [NH4+] if SO42–/NH4+ > 1.
c – [ex-NH4+] = [NH4+] – 0.27[(NH4)2SO4].
d – [NH4NO3] = 4.44[ex-NH4+].
prove that some anions in PM were not
neutralized. They show that the determined main dust components constituted only a part of the total PM mass.
It is probable that the insoluble fractions
of Ca, Mg or K (not analysed in this
study) as well as other elements, mainly
H (component of nitric and sulphuric acids) balanced the anions occurring in the
aerosol.
The particles with a diverse fraction
composition, with the predominant mass
percentage of coarse particles (Pierson
and Brachaczek 1983, Allen et al. 2001),
are emitted as a result of the mechanical wear of the materials used to produce
cars and harden road surfaces. The road
surfaces also make a significant source
of the secondary emission (usually coarse
particles), particularly in the periods
without precipitation and in winter, when
chemical substances are used to prevent
the black ice (e.g. Pastuszka et al. 2010).
Importantly, these findings explain the
visibly higher K, Ca, Na and Cl concentrations in the coarse PM, which occurred
at the A4 point (Fig. 1, Table 1).
249
The sum of the identified PM components constituted between nearly
58% (PM2.5-10) and approximately 73%
(PM1-2.5) of the PM mass at the A4 sampling point. In the urban background
(TM), the determined PM components
helped to reconstruct between 56%
(PM2.5-10) and 71% (PM1-2.5) of the
PM mass (Fig. 2). The coarse PM at
the urban background point contained
considerably more primary matter. It
mainly concerned primary organic matter (OMprim). The same PM fraction
collected at the motorway contained significantly more secondary organic matter
(OMsec), i.e. matter formed as a consequence of the transformation reaction of
the gas precursors into particles (Castro
1999, Seinfeld and Pandis 2006). On the
other hand, there was more OMsec in
the fine and submicron PM at the urban
background (TM).
In general, the PM mass at the motorway contained between 30 (PM2.5-10)
and 60% (PM1-2.5) of the secondary
compounds – OMsec, NH4NO3 and
(NH4)2SO4). The remaining part of the
OM – organic matter (OM = 1.4×OC); the division of OM into OMsec and OMprim was based on the
scheme discussed in the study (Rogula-Kozłowska et al. 2013); the NH4NO3 and (NH4)2SO4 concentrations were assumed in accordance with the results given in Table 2.
FIGURE 2. Mass reconstruction of three PM fractions at the traffic sampling point at the motorway
(A4, on the left) and at the urban background point (TM, on the right) in Katowice
250
identified PM mass was composed of
primary compounds (OMprim, EC, Na +
+ Cl and K + Ca + Mg). At the urban
background point, the secondary aerosol
– both organic (OMsec) and inorganic
one (NH4NO3 and (NH4)2SO4) – made
up between 20 (PM2.5-10) and 60% (PM1
and PM1-2.5) of the PM mass (Fig. 2).
The discrepancies between the PM
mass and the sum of its components arise
from the fact that a group of compounds
that were not chemically analysed occurred in the dust (a number of elements,
carbonaceous and/or organic anions).
The lack of the so-called complete mass
closure (mass reconstruction) can be
also related to the evaporation of the organic compounds and nitrates during the
transport and storage of the PM samples
(particularly in warm and dry periods).
The presence of water bound to the PM
particles is a very important factor that
exerts impact on the chemical balance
of the PM mass. The study (Tsyro 2005)
demonstrates that the water percentage
under the 50-percentage RH conditions
varies in different European areas. It can
constitute 20–35% of the PM2.5 mass.
Additionally, the results of the chemical
reconstruction of the PM mass are also
influenced by the errors and measurement uncertainty related to each research
stage (sampling, gravimetric and chemical analyses).
CONCLUSIONS
The PM concentrations and components
were determined for three selected PM
fractions (submicron, fine and coarse) at
two sampling points, i.e. the A4, located
at the motorway, and the TM, placed
in the so-called urban background. The
analysis did not indicate any particular
differences between the parameters investigated at both points.
The differences in the PM concentrations were visible only for the coarse
PM fraction as they were higher by 25%
at the A4 point than at the TM one. The
differences in the PM chemical composition were slight at both points. There
was definitely more EC in the city centre
at the motorway. At this spot, the coarse
PM fraction contained more OMsec,
whereas its content in the submicron PM
fraction was undeniably lower than at
the urban background point. On the other hand, there were more primary components related to the resuspension and
other mechanical processes (i.e. wear/
/erosion of the materials used to produce
cars and harden the road surfaces) in the
coarse PM mass at the motorway.
The analysis of the obtained results
confirms that the traffic emission can
have a less significant influence on the
concentrations and chemical composition of the three analysed PM fractions
in Katowice than in other European regions.
Acknowledgments
The work was realized within the projects
C.1.2. and N N523 564038, the former
financed by the Institute of Environmental Engineering, PAS, the latter-by the
Polish Ministry of Science and Higher
Education.
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Streszczenie: Wpływ ruchu drogowego na stężenia trzech frakcji pyłu zawieszonego (PM) i jego
główne składniki w dużym mieście Górnego Śląska. W pracy oceniono wpływ ruchu drogowego
na stężenia trzech frakcji pyłu i ich podstawowych
składników. Próbki pyłu pobrano równolegle
w parze receptorów w Katowicach. Jeden z punktów pomiarowych zlokalizowany w punkcie tzw.
tła miejskiego; drugi reprezentował tzw. punkt
komunikacyjny. W próbkach oznaczono zawartość węgla organicznego i elementarnego oraz jonów rozpuszczalnych w wodzie. Stwierdzono, że
w typowym obszarze miejskim południowej Pol-
253
ski wpływ emisji zanieczyszczeń z silników samochodowych ujawnia się w przypadku pyłu submikronowego i drobnego poprzez wzbogacenie
ich cząstek w węgiel elementarny. Wpływ resuspensji pyłu drogowego i glebowego wywołanej
ruchem samochodowym na kształtowanie stężeń
i składu chemicznego widoczny jest natomiast
w przypadku frakcji pyłu grubego.
Słowa kluczowe: PM1, PM1-2,5, PM2,5-10, węgiel
elementarny, węgiel organiczny, skład chemiczny,
rozkład frakcyjny, stanowisko komunikacyjne, tło
miejskie
MS. received in December 2013
Authors’ address:
Instytut Podstaw Inżynierii Środowiska PAN
ul. M. Skłodowskiej-Curie 34
41-819 Zabrze, Poland
e-mail: [email protected]
[email protected]
[email protected]
[email protected]

INTRODUCTION Effects of road traffic on the ambient concentrations

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